Influence of Cellulose Filaments on Cement

Paste and Concrete

Ousmane A. Hisseine 1; Ahmed F. Omran 2; and Arezki Tagnit-Hamou 3

Abstract: In light of the current increasing interest toward nanomaterials for concrete technology, it appears that nanocellulose (with its
incredible properties) can shape a promising sustainable candidate. This study investigates the influence of a new type of nanocellulose
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materials, namely, cellulose filaments (CF), on the properties of cement pastes and self-consolidating concrete (SCC). CFs were found
to alter mixture rheology and improve its stability because of the filaments’ hydrophilicity. While the compressive strength of CF pastes
was adversely affected (because of air entrainment and filament agglomeration), the flexural capacity was increased by up to 25%. In SCC, all
measured mechanical properties were enhanced. Strength improvements of up to 16% (in compression), 34% (in splitting tension), 22% (in
flexure), and 96% (in energy absorption) were obtained. These improvements were attributed to two effects imparted by CF: nanoreinforcing
and internal curing. The former was evidenced by microstructural analysis, while the latter was confirmed by the assessment of autogenous
shrinkage, in which CF reduced the shrinkage strains at 7 days by up to 31%. In SCC, CFs also imparted a viscosity-modifying effect,
in which the hardened properties were enhanced via improving mixture stability. DOI: 10.1061/(ASCE)MT.1943-5533.0002287.
© 2018 American Society of Civil Engineers.
Author keywords: Cement paste; Cellulose filaments; Mechanical performance; Microstructure; Nanocellulose; Self-consolidating
concrete (SCC) rheology.

Introduction alternative reinforcement. Unfortunately, many untreated NFs

exhibit durability issues, inconsistency in properties, and poor ad-
In the context of sustainable development, the concrete technology herence to the matrix (Romido et al. 2000). NFs are very effective in
community has been striving constantly to enhance the performance controlling plastic shrinkage [e.g., 99% reduction in crack width
of concrete in different dimensions with a particular focus on eco- and total crack area with only 0.3% by volume (Boghossian and
efficiency perspectives. Fiber-reinforced concrete (FRC) technol- Wegner 2008)], mitigating drying shrinkage [e.g., 86% reduction
ogy is one of the major leaps in this quest, which has led to concretes in crack width with only 1% by volume (Kawashima and Shah
with enhanced tensile strength, ductility, toughness, and fatigue re- 2011)], and improving the mechanical performance of cement com-
sistance (Banthia et al. 1994; Khaloo and Afshari 2005; Altoubat posites [e.g., 20–50% enhancement in flexural strength and fracture
et al. 2016). Nonetheless, there are several concerns about fibers toughness when a NF dosage of 2–16% by weight was considered
conventionally used in FRC. These concerns include low corrosion (Sedan et al. 2008; Morton et al. 2010; Merta and Tschegg 2013)].
resistance in steel fibers (Kosa and Naaman 1990), poor bond with Nevertheless, the industrial production of NF concrete is currently
the cementitious matrix and degradability under cement’s alkaline limited. This is due primarily to the inconsistence in fiber properties
medium in glass fibers (Rybin et al. 2016), and low cost effective- leading to variations in concrete performance. The variation in con-
ness in carbon and polymer fibers (Chung 2000). In this respect, crete performance hinders an accurate prediction of mechanical
since cellulose is considered to be the most ubiquitous and behavior (Aziz et al. 1981). Additionally, NFs exhibit another
renewable natural polymeric raw material on the planet, it may be handicap, which is the fibers’ vulnerability in the cement’s alkaline
legitimate to believe that plant-based natural fibers (NF) have medium (Ardanuy et al. 2011). This is attributable to the alkaline
the potential to offer the most cost-effective and sustainable degradation of some fiber components such as lignin, hemicellu-
lose, pectin, and soluble sugars (Onuaguluchi and Banthia
1 2016). The advantages offered by NFs could have been optimized
Ph.D. Candidate and NSERC Canada Vanier Scholar, Cement and
Concrete Research Group, Dept. of Civil Engineering, Université de
if some of these issues were addressed.
Sherbrooke, 2500, Blvd. de l’Univ., Sherbrooke, QC, Canada J1K 2R1 Recently, research works in nanoscale plant-based materials
(corresponding author). E-mail: [email protected] have led to the emergence of what is called nanostructured
2
Research Professional, Dept. of Civil Engineering, Université de cellulose. This includes an array of cellulosic materials such as
Sherbrooke, 2500, Blvd. de l’Univ., Sherbrooke, QC, Canada J1K 2R1; nanofibrillated cellulose (NFC), cellulose nanocrystals (CNC), bac-
Assistant Professor, Univ. of Minoufiya, Gamal Abd El-Nasir St., Shibin terial cellulose (BC), and cellulose filaments (CF). NFC consists of
El-Kom, Menoufia 32511, Egypt. E-mail: [email protected] alternating crystalline and amorphous domains made of bundles of
3
Professor and Head of the Cement and Concrete Research Group, stretched cellulose chain molecules with long, flexible, and en-
Dept. of Civil Engineering, Université de Sherbrooke, 2500, Blvd. tangled cellulose nanofibers of approximately 1–100-nm diameter
de l’Univ., Sherbrooke, QC, Canada J1K 2R1. E-mail: A.Tagnit@
and 500–2,000-nm length (Moon et al. 2011). CNC consists of rod-
USherbrooke.ca
Note. This manuscript was submitted on May 18, 2017; approved on like highly crystalline cellulose particles of 2–20-nm diameter and
November 22, 2017; published online on April 10, 2018. Discussion period 50–500-nm length, thereby exhibiting a lower aspect ratio com-
open until September 10, 2018; separate discussions must be submitted for pared to NFC and a limited flexibility due to the absence of amor-
individual papers. This paper is part of the Journal of Materials in Civil phous portions (Brinchi et al. 2013). BC particles are microfibrils
Engineering, © ASCE, ISSN 0899-1561. secreted by various bacteria and have different morphologies, but

© ASCE 04018109-1 J. Mater. Civ. Eng.

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 they are typically rectangularlike, 6–10 nm wide and 30–50 nm The influence of CF on fresh and rheological properties, heat of
long (Eichhorn et al. 2010). CFs are mechanically processed hydration, early-age deformations, microstructure, and mechanical
cellulose fibrils with micrometric length and nanometric diameter. performance was examined. For the cement pastes, the mechanical
CFs exhibit some structural similarities with NFC, but they have an performance was evaluated in a function of the curing regime (moist
extended length (100–2,000 μm) compared to their diameter (30– versus sealed) in order to disclose the effect of CF on internal curing.
400 nm), thereby resulting in a significantly higher aspect ratio
(100–1,000). The treatment of natural fibers at the nanoscale to
yield these nanostructured cellulose particles increases the consis- Experimental Program
tency in their material properties (lacking at the macroscale) and
removes fibers’ degradable compounds. Additionally, the use of
Materials Properties
nanostructured cellulose can allow exploitation of the power of
cellulose polymers that imparts inherent strength to plants through Four cement pastes and four SCC mixtures were considered in this
the complex hierarchical structure of cellulose. The incorporation study. Type General Use (GU) cement and Class F fly ash (FA) with
of nanocellulose into cement systems has the further potential to Blaine fineness values of 431 and 287 m2 =kg, respectively, were
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obtain what is called nanomodified concrete (Jongvisuttisun used. The chemical composition determined by X-ray fluorescence
et al. 2013). for the cement includes 20.5%SiO2 , 4.0%Al2 O3 , 2.0%Fe2 O3 ,
Nanomodification of concrete refers to incorporating nanosized 63.2% CaO, 2.2% MgO, 3.4%SO3 , and 1.1%Na2 Oeq . For FA,
objects into concrete to manipulate its nanostructure and control its the chemical composition includes 53.7%SiO2 , 17.5%Al2 O3 ,
macro behavior (Jennings et al. 2008) in order to develop a new 5.6%Fe2 O3 , 12.4% CaO, 2.1% MgO, 1.4%SO3 , and 3.6%Na2 Oeq .
generation of tailored and multifunctional composites with superior The CF used in this study was manufactured and provided by
mechanical performance and durability (Sanchez and Sobolev Kruger Biomaterials (Trois-Rivières, Québec, Canada) in a semi-
2010). Published studies on nanomodification of concrete have dispersed form (a nominal moisture content of 70%). The filaments
hitherto covered nanometal oxides (e.g., nanosilica, nanotitanium were extracted from wood pulp through a process (patent pending)
dioxide, nanoiron oxide, nanoalumina, etc.); nanoclay; carbon that uses only mechanical energy. Generally, wood pulp is made of
nanofibers; and carbon nanotubes. Relevant investigations on nano- a large amount of cellulose macrofibers. The wall structure of cel-
structured cellulose are scarce. Whereas the incorporation of nano- lulose macrofibers is composed of bunches of closely stacked cel-
cellulose in polymer matrices is deep rooted (Boldizar et al. 1987; lulose macrofibrils organized around a cavity called a fiber lumen.
Favier et al. 1995; Dufresne and Vignon 1998; Al Turaif 2013), its A single cellulose macrofibril is composed of tiny bands of cellu-
applications in cement and concrete composites are still nascent. lose microfibrils, which, when peeled axially, create CFs. CFs re-
Our survey of literature has indicated that very few investigations present an intrinsic part of the hierarchical structure of cellulose
have reported on the incorporation of NFC, NCC, and BC in ce- (Fig. 1), which imparts intrinsic strength to plant-based materials.
ment composites. The extraction process of CF involves the removal of matrix impu-
In general, the available literature on the use of nanostructured rities such as lignin, pectin, wax, and soluble sugars. As a result, CF
cellulose in cement composites indicates influences on hydration contains mainly cellulose (>95%) and a small amount of hemicel-
kinetics, rheological properties, and mechanical performance. lulose (<5%). This is consistent with the two types of saccharides
Reported effects on hydration kinetics include a reduction in mix- (glucose and xylose) detected by liquid chromatography tests con-
ture conductivity, impediment of early-age hydration kinetics, and ducted on CF. Typically, the former is found in cellulose, while the
acceleration of the hydration process at later ages (Jongvisuttisun latter is found in hemicellulose.
et al. 2013). The influences on rheological properties include an To prepare CF suspensions (with different CF concentrations),
increase in viscosity and yield stress in a shear thinning behavior the as-received CF material was added to the mixing water and
(Gómez et al. 2013; Cao et al. 2015), an increase in water and homogenized by high shear mixing. Fig. 2 shows pictures of water
superplasticizer demands, and a decrease in workability (Peters suspensions with varying CF contents, while Figs. 3 and 4 depict
et al. 2010). Nanostructured cellulose also alters the microstructure field emission gun-scanning electron microscopy (FEG-SEM)
of cement composites and influences their mechanical perfor-
mance. Onuaguluchi et al. (2014) reported increases in flexural
strength and energy absorption of cement pastes containing 0.1%
by weight NFC by approximately 106 and 184%, respectively. Cao
et al. (2015) reported improvement in flexural strength of 20–30%
at an optimum CNC dosage of 0.2% by weight due to an enhanced
degree of hydration. Peters et al. (2010) found that a NFC addition
of 0.5% by weight was optimal for improving the fracture proper-
ties of ultrahigh-performance concrete. Despite several common
features between existing nanocellulose materials and the CFs in-
vestigated herein, CFs exhibit the highest aspect ratio owing to their
micrometric length but nanometric diameter. Initial applications of
CF emerged in the paper and pulp industry, where the strength of
sheets made from Kraft pulp was improved by 250% at the addition
of 10% CF [X. Hua, M. Laleg, K. Miles, R. Amiri, L. Ettaleb, and
G. Dorris, “High aspect ratio cellulose nanofilaments and method
for their production,” U.S. Patent No. 9051684 B2 (2015)]. The
incorporation of CF in cement systems is a new endeavor addressed
in this study, in which the effect of CF at dosages of 0.1, 0.15, and
0.2% by weight on the fresh and hardened properties of paste
Fig. 1. Schematic of hierarchical structure of cellulose filaments (CFs)
and self-consolidating concrete (SCC) mixtures was investigated.

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Fig. 2. Cellulose filament (CF): (a) in a semidispersed form, as received; (b) in aqueous suspensions used to prepare the mixes

Fig. 3. SEM image of a dried diluted CF aqueous suspension with Fig. 4. SEM image of a dried diluted CF aqueous suspension with
0.1% CF: CF network 0.1% CF: individual fibrils

images of a dried CF diluted suspension with 0.1% CF. The figures Table 1. Concrete Mix Proportions
illustrate the fibrillar morphology for a network of filaments (Fig. 3) Component Ref. 0.1% CF 0.15% CF 0.2% CF
and for some individual fibrils (Fig. 4). 3
Cellulose filament (kg=m ) — 0.487 0.731 0.974
In the SCC mixtures, crushed limestone coarse aggregates with Type GU cement (kg=m3 ) 365
5–14 mm maximum size, 2.77 specific gravity, and 0.52% water Class F fly ash (kg=m3 ) 122
absorption rate were used. Natural river sand with a specific Total binder (kg=m3 ) 487
gravity of 2.65 and an absorption rate of 0.9% was employed. Water (kg=m3 ) 200
A polycarboxylate-based high-range water-reducing admixture W=B 0.42
(HRWRA) with 32% solid content—fulfilling the requirements Sand, 0–5 mm (kg=m3 ) 804
of ASTM C494 Type F admixtures (2016a)—was added at a con- Coarse aggregate, 825
stant dosage of 2.5 L=m3 to secure the target flowability of 750 mm 5–14 mm (kg=m3 )
HRWRA (L=m3 ) 2.5
in the plain SCC mixture.
Note: Ref. = reference mixture.

Mixture Proportions and Mixing Procedures

relevant section. All paste mixtures were prepared following the
Four paste mixtures were designed with cement: FA: water propor- ASTM C305 guidelines (ASTM 2014a).
tions of 1.00: 0.33: 0.50 by mass, respectively. The mixtures con- Four SCC mixtures were designed with a water-to-binder ratio
tain, respectively, 0, 0.1, 0.15, and 0.2% by weight CF. FA was (W=B) of 0.42: a reference mixture with no CF (designated in this
incorporated in pastes to be consistent with the SCC systems in- manuscript as Ref.) and three mixtures incorporating CF at dosages
vestigated in parallel. The above mixtures were used in all tests of 0.1, 0.15, and 0.2% by weight of binder (Table 1).
conducted on pastes, excluding autogenous shrinkage, where a An aqueous suspension of CF was prepared by diluting the as-
slightly different recipe was adopted and detailed later in the received material into water by applying high shear mixing for 60 s

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 Table 2. Mixing Procedure were regularly measured during a period of 18 h until the mass loss
System Mixing procedure stabilized at a final mass of 1.7
0.02 g. This corresponds to 34%
of the initial 5.0 g mass. To examine the possible effects of the
Pastes Add mixing water in the form of CF suspension.
filament’s MC on the mixing water during the preparation of pastes
Add cement (and fly ash) to the water and allow 30 s for
water absorption.
and concretes, a set of CF samples of 0.3 g were subjected to cen-
Mix at low speed for 30 s. trifugation at 2,000; 3,000; and 4,000 rpm. For each centrifugation
Stop the mixer for 15 s; scrape during this time. speed, the mass loss was evaluated after 10, 20, and 30 min of
Mix at medium speed for 60 s. centrifugation. The water retention capacity (WRC) of CF was de-
Concretes Add aggregate and sand, mix for 1 min. termined using the following methodology: A 30.0 g sample of as-
Add the first half of water containing CF, mix for 1 min. received CF was kept in an oven at 60°C until a final mass of 10.2 g
Add cement (and fly ash), mix for 0.5 min. of dry CF (34% of the initial mass) was obtained. Several CF sus-
During mixing at above step, add the second half of water, pensions were prepared by mixing 0.1 g of dry CF (referred to
continue mixing for 2.5 min. herein as M0 ) with 1.9 g of distilled water. The well-tight samples
Pause for 2 min to allow air bubbles to evacuate.
were then stored at 22°C and 50% RH until tested at predetermined
Remix for 2 min; then start casting.
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water immersion durations (i.e., 1, 3, 6, 12, 24, 48, or 72 h). For

each water immersion duration, four samples were subjected to
centrifugation at 3,000 rpm for 25 min using 2-mL centrifugal fil-
using a 700-watt blunt-blade blender. CF disintegration was carried ters of 100,000 molecular weight cutoff (MWCU) to drain out
out for 10 s at a low speed (100 rps); 20 s at a moderate speed water. The resulting CF was accurately weighted for its wetted
(200 rps); and 30 s at a high speed (300 rps) in an attempt to mass (M 1 ) and the WRC was determined as
disentangle filament clumps. To attenuate filament damage during  
mixing, the blender was carefully selected so as to have a two-tip M1 − M0
WRC ¼ × 100% ð1Þ
horizontally laid blade with blunt (less sharp) edges. This was an M0
attempt to foster the disintegration of filaments by the resulting ro-
tational energy created in the suspension rather than by the blades’ To evaluate the water release rate (WRR) of CF, after the WRC
torque alone. The above dispersion protocol was adopted by the test, the samples for 72-h immersion were exposed to 38
1°C and
authors upon investigating the effectiveness of other strategies, 20
1%RH. The samples were then accurately weighed and their
namely, magnetic-field shearing, ultrasonication, and dispersion mass (M 2 ) after moisture loss was recorded after a series of expo-
with surfactants. sure durations (0.17, 0.5, 2, 3, 4, 8, 12, 16, 20, 24, and 48 h).
For paste mixtures where no HRWRA was used, the resulting The WRR was calculated as follows:
CF suspension was then added to the total adjusted mixing water.  
For SCC mixtures, a HRWRA was added to the adjusted mixing M1 − M2
WRR ¼ × 100% ð2Þ
water, and the resulting suspension was split into two halves, M1 − Mo
one of which was mixed with the CF suspension. The ensuing
mixture (CF-water-HRWRA) was homogenized by shaking the
suspension for approximately 30 s. This step could have also been Tests on Paste Mixtures
carried out by stirring since it is simply an extra precaution for an
already dispersed CF suspension. Paste systems were prepared us- Fresh and Rheological Properties. The fresh properties of pastes
ing a Globe SP20 mixer, while the SCC mixtures were prepared included the mini-slump-cone test [ASTM C230 (ASTM 2014b)],
using a Crown C9 concrete mixer. Detailed mixing procedures the mini-V-funnel test (EFNARC 2005), the air content [ASTM
for pastes and concrete mixtures are described in Table 2. C185 (ASTM 2015)], and the temperature. In the mini-slump-cone
test, the spreading diameter was measured immediately after cone
lifting and also after subjecting the sample to 25 blows from the
Samples’ Curing and Testing Procedures flow table. Moreover, the rheology of all paste mixtures was as-
The influence of two curing regimes (moist versus sealed) on the sessed using a coaxial-cylinder rheometer with a serrated surface
mechanical properties was investigated for paste mixtures. This and cup and bob diameters of 28.911 and 26.660 mm, respectively,
was intended to assess the potential effect of CF on internal curing. providing a shear gap size of 1.126 mm.
For moist curing, the paste specimens were kept in a curing room Isothermal Calorimetry. The heat evolution in all paste
at 100% relative humidity (RH) and 22°C until the time of testing. mixtures was monitored using a TAM air isothermal calorimeter
In the sealed curing condition, the paste specimens were hermeti- (TA Instruments, New Castle, Delaware) following the guidelines
cally wrapped with adhesive plastic sheets and kept in a controlled of ASTM C1702 (ASTM 2017). From each mixture, a 3.0 g sample
medium (50% RH and 22°C) for 7 days, followed by unwrapping was placed into a calorimetric chamber (kept at a constant temper-
and storing the specimens in the same environment for an addi- ature of 22
0.1°C). Measurements were collected for a continu-
tional 21 days. ous period of 28 h and were used to assess the effect of CF on the
For concrete mixtures, upon casting, samples were stored in a heat evolution of different paste mixtures.
room with a RH and temperature of approximately 50% and 23°C, Autogenous Shrinkage. Autogenous deformations were measured
respectively, for 24
1 h. Then they were demolded and transferred to assess the potential effect of CF on internal curing. A plain paste
for storage in a fog room at 100% RH and 22°C temperature until mixture and three mixtures containing CF (at 0.1, 0.15, and 0.2%
the age of testing. The different test methods adopted to execute the CF) were considered for this purpose. As is well known, autog-
experimental program are elaborated in the following sections. enous shrinkage occurs in all cement composites, but it is more
evident in systems with a low water-to-cement (W=C) ratio
Tests of Moisture Content and Water Retention/Release (Tazawa and Miyazawa 1995). Therefore, paste mixtures with a
Capacity of CF slightly lower W=C (0.35) were designed to mobilize autogenous
The moisture content (MC) of the as-received CF was determined shrinkage so that the potential effect of CF on this phenomenon can
on five samples of 5.0 g mass kept in an oven at 60°C. The samples be better captured. The reduction of W=C, however, necessitated

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 the introduction of a water reducer to maintain mixture flowability deformations. This is because, prior to the final setting time, as
(a mini-slump flow diameter of 250
15 mm). A HRWRA with a the paste is still plastic, deformations are predominantly due to
dosage of 0.25% by weight of cement was introduced on a solid (1) the chemical shrinkage resulting from the vigorous exothermal
basis. This dosage was slightly increased to 0.27, 0.30, and 0.35% reactions accompanying the hydration of the cement’s active phases
by weight in the specimens with 0.1, 0.15, and 0.2% CF, respec- and (2) the potential deformation of the strain gauge itself due to the
tively. Paste prisms measuring 80 × 80 × 350 mm were instru- rise of temperature as the cement hydrates. Moreover, the splitting-
mented with embedded vibrating-wire strain gauges of type tensile strength (f sp ) was evaluated on 100 × 200 mm paste cylin-
EM-5 (Roctest, Saint-Lambert, Québec, Canada) of 144 Ω resis- ders at 1, 3, and 7 days in accordance with ASTM C496 guidelines
tance and a strain range of 3,000 με [Fig. 5(a)]. Additional to meas- (ASTM 2011) in an attempt to unveil a reinforcing action of CF,
uring deformations resulting from autogenous shrinkage, if any.
the gauge is also equipped with a thermocouple to record temper- Mechanical Properties. Specimens for mechanical properties
ature evolutions in the paste throughout the testing period were sampled from each paste mixture soon after mixing and then
so that temperature-borne deformations can be subtracted from demolded 24
1 h later. For each paste mixture, cube samples
the total deformation. To ensure full embedment of the gauge in (50 × 50 × 50 mm) and prisms (50 × 50 × 160 mm) were pre-
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the paste, the gauge was set centered in the mold (in all directions) pared to assess the mechanical performance. The cubes were tested
using attachment wires so as to allow it a free rotation and axial for compressive strength (f c ) at 1, 7, and 28 days according to
translation (necessary to respond to the matrix linear deformations). ASTM C109 guidelines (ASTM 2016c), while the prisms were
The fresh cement pastes were placed in the mold in two layers and tested for flexural capacity (ffl ) at 28 days according to ASTM
were consolidated following the procedures detailed in ASTM C348 guidelines (ASTM 2014c). Mechanical properties at all ages
C157 (ASTM 2014d). The molds containing the pastes were her- (under both curing regimes) were tested on a minimum of three
metically sealed with adhesive plastic wraps immediately after cast- samples. The average value was used to compare the performance
ing and remained so until demolded 24
0.5 h later. Immediately of different mixtures.
after demolding (within 2
1=2 min), the specimens were sealed Microstructural Analysis. A high-resolution field emission gun
with an adhesive aluminum foil and kept in a controlled environ- (FEG) scanning electron microscopy (SEM) of type Hitachi
ment (50% RH and 22°C) for 7 þ days [Fig. 5(b)]. Data were auto- S-4700 (Tokyo, Japan) equipped with an Oxford energy dispersive
matically recorded via an acquisition system at a 30 min frequency spectroscopy (EDS) of type X-Max (Oxford Instruments, Abing-
during the first day and 4 h frequency thereafter. don, United Kingdom) was employed to analyze the microstructure
Parallel to the measurements of autogenous deformations, of cement pastes. Analysis was conducted on fresh fractured sur-
the setting time of the tested paste mixtures was determined by faces to promote the visibility of CF. Test specimens were coated
the Vicat needle test [ASTM C191 (ASTM 2013)]. The final setting with gold palladium for 60 s to assuage the effect of surface charges
time was used as a datum for the readings of autogenous induced by the ultrahigh-energy electron beam. A double-faced ad-
hesive carbon film was placed between the specimen and the
specimen-holding plate to foster conductivity. A secondary electron
(SE) detector, operated at 2.0 or 3.0 kV accelerating voltage and an
emission current of 10 μA, was adopted for the analysis of the frac-
tured specimens.

Tests on Concrete Mixtures

Fresh and Rheological Properties. For the concrete mixtures, the
assessment of fresh properties was carried out using common SCC
fresh property tests, which included (1) the slump-flow diameter,
the time required to reach a 500 mm spread diameter (T 500 ), and the
visual stability index (VSI) [ASTM C1611 (ASTM 2014f)]; (2) the
J-ring spread diameter and blockage ratio [ASTM C1621 (ASTM
2014e)]; and (3) the V-funnel (EFNARC 2005).
The rheology of concrete mixtures was assessed using a ConTec
5 rheometer (Contec, Laugarasvegur, Iceland), which consists of a
fixed outer cylinder and an inner rotating bladed cylinder. The ro-
tation speed was adjusted to increase from 0.025 to 0.5 rps in 10
points such that 50 resistance-time measurements were recorded at
each point. For the analysis of the rheological measurements, the
Bingham model (Bingham and Reiner 1933) was adopted to char-
acterize the mixture flow behavior by measuring the rheology data
such as yield stress (τ 0 ), plastic viscosity (μpl ), shear stress (τ ), and
0
shear rate (γ ).
Mechanical Properties. For each concrete mixture, the f c [ASTM
C39 (ASTM 2016b)] at 1, 7, and 28 days and f sp [ASTM C496
(ASTM 2011)] at 28 days were measured using 100 × 200 mm cyl-
inders. The f fl [ASTM C78 (ASTM 2016d)] and the flexural tough-
ness (T b ) were evaluated using 100 × 100 × 400 mm prisms (at
28 days). The flexural tests were performed under a four-point bend-
Fig. 5. Test setup for autogenous shrinkage: (a) mold with an em-
ing configuration in a displacement-controlled mode using a dis-
bedded vibrating-wire strain gauge; (b) specimens sealed with adhesive
placement rate of 0.0008 mm=s. T b was determined following
aluminum foil and connected to a data acquisition
the JSCE SF-4 approach (JSCE 1984), where T b is defined as

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 the area under the load-deflection curve until a deflection of 1=150 of
span. It is also defined alternatively as the area immediately before
failure if the specified deflection is not reached. The area under the
load-deflection curve from flexural testing was calculated using the
Trapz built-in function in MATLAB.
Microstructural Analysis. The microstructural investigations on
concrete mixtures were carried out on fresh fractured concrete sam-
ples at the age of 28 days following the same testing techniques
adopted for paste mixtures described earlier.

Results of Tests for CF Moisture Content and Water

Retention/Release
Fig. 8. Water release rate of CF in a function of the duration of
exposure to a dry medium
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Results of the MC of CFs are presented in Fig. 6. The moisture loss

at 60°C was very steep in the first 4 h and then stabilized thereafter
until the mass of the dry CF became constant (at 34% of the initial
20
1%RH) and plateaued at 96.8% in 48 h. Whereas this trend
mass) beyond 18 h. The MC of CF at the time of preparing the paste
gives an indication of the water desorption of CF, a more compre-
and concrete mixtures can be taken as 66%. However, this sus-
hensive assessment would examine the WRR under variable RH,
pended water was not considered in calculating the mixing water.
particularly at higher RH.
In fact, as mentioned earlier, a series of tests were conducted to
examine the possible effect of the filament’s MC on the mixing
water. These tests showed that upon subjecting the as-received
material to centrifugation at 2,000; 3,000; and 4,000 rpm (for Results and Discussion for Paste Mixtures
up to 30 min), no mass loss was recorded at all.
The results of the WRC of CF are shown in Fig. 7. The figure Fresh Properties and Rheology
shows that within 1 h of saturation in water, CF can imbibe up to The fresh properties of all paste mixtures are presented in Table 3.
80% of its mass. The WRC exceeds 100% by 6 h of saturation and The results show that CF significantly altered mixture workability.
stabilizes at 125% when CF was saturated for 72 h. CF samples Whereas the slump-flow diameter (before shocking) was 160 mm
obtained from WRC tests at 72 h of saturation followed by centrifu- in the reference paste, the incorporation of CF at dosages of 0.1,
gation at 3,000 rpm for 25 min released their absorbed water 0.15, and 0.2% reduced the slump flow diameter to 100, 90, and
according to the trend shown in Fig. 8. The WRR of CF exceeded 85 mm, respectively. After 25 blows on the flow table, the reference
50% by 4 h of exposure to a dry medium (38
1°C and paste had a flow diameter of 330 mm, while the incorporation of CF
at dosages of 0.1, 0.15, and 0.2% reduced the slump flow diameter
to 290, 270, and 240 mm, respectively. The decrease in workability
exhibited in mixtures with CF was directly reflected by a remark-
ably higher V-funnel passing time. From 3.50 s passing time in the
reference mixture, the incorporation of CF at 0.1, 0.15, and 0.2%
augmented the passing time to about 13, 25, and 42 s, respectively.
This corresponds to about 4, 7, and 12 times the passing time of the
reference paste. These observations indicate a significant reduction
in workability when CF is used. This is further evidenced by the
results in Fig. 9 for the rheological measurements of the plain paste
mixture and the mixtures with 0.1 and 0.15% CF. The mixture with
0.2% was not tested as its viscosity was beyond the device limit.
Fig. 9 indicates that the incorporation of CF at a dosage of 0.15%,
Fig. 6. Moisture content in CF; the figure shows the mass loss at 60°C for instance, increased the yield stress and the plastic viscosity of
the reference paste by 35 and 42%, respectively. This can be re-
flected by an increased mixture cohesion and homogeneity and
can be attributed to the hydrophilic nature of CF and to its nano-
metric fibrillar structure. The hydrophilicity of CF leads to water

Table 3. Fresh Properties of Paste Mixtures

Slump flow
diameter
V-funnel
(mm)a
Temperature Air content passing
Paste mixture (°C) (%) Before After time (s)
Ref. 26.0 0.68 160 330 3.50
0.1% CF 27.5 1.16 100 290 13.21
0.15% CF 29.3 1.87 90 270 25.42
0.2% CF 29.7 2.18 85 240 42.13
Fig. 7. Water retention capacity of CF in a function of the duration of a
Slum flow was measured before and after subjecting the specimen to 25
saturation in water
blows on the flow table.

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 materials with high purity in cellulose and has been reported in a
more pronounced manner in cellulose-based polymers (Mishra
et al. 2003), microcrystalline cellulose (Gómez et al. 2013), cellu-
lose nanofibers (Onuaguluchi et al. 2014), cellulose nanocrystals
(Cao et al. 2015), and bacterial nanocellulose (Mohammadkazemi
et al. 2015). The increased heat of hydration observed in CF mix-
tures can be linked to the alkaline hydrolysis of cellulose, which is
an exothermic reaction that promotes cement hydration and leads to
a sort of acceleration (Knill and Kennedy 2003). This is further
confirmed by the reduced setting time recorded in CF-SCC mix-
tures investigated in parallel.
Fig. 9. Rheological measurements of cement pastes

Autogenous Shrinkage
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adsorption whereby water molecules adhere peripherally to CFs, Table 4 presents some of the fresh and hardened properties for the
thereby fixing some of the mixing water. This is confirmed by pastes considered for autogenous shrinkage. Results from the Vicat
the water absorption capacity of CF described in the previous sec- setting time indicate that mixtures with CF exhibited some slight
tion where CF can imbibe water up to 80% of its mass within 1 h retardation. Referring to the aforementioned results of isothermal
and more than 100% of its mass by 6 h. Additionally, the nanomet- calorimetry where mixtures with CF exhibited slightly higher heat
ric fibrillar structure, flexibility, and high aspect ratio of CF pro- release, the retardation experienced herein may be attributable to
mote the intertwining and entanglement of individual filaments the effect of HRWRA. While the increasing dosage of HRWRA
and/or the formation of filament networks, which can increase in pastes with CF enabled attaining the target slump flow diameter
mixture viscosity and enhance its stability. Such effects on mixture of 250
15 mm, it may have been responsible for the observed
flow and rheology have also been observed in some polysaccharide retardation. Such effects are well reported for increasing dosages
of polycarboxylate-based HRWRAs (Zingg et al. 2009).
viscosity-modifying agents (VMAs) with a microbial source, such
Results of autogenous shrinkage measurements showed that the
as welan gum (Khayat 1995). On the other hand, whereas the ad-
incorporation of CF altered the early-age deformations in the
dition of CF increased the viscosity, it was observed that mixtures
cementitious matrix. Fig. 11 shows that paste mixtures with CF
with CF exhibited higher air content. For the three tested CF dos-
exhibited lower autogenous shrinkage at all ages. At 7 days, for
ages (0.1, 0.15, and 0.2%), the amount of entrapped air was respec-
instance, the reference paste recorded a shrinkage strain of 366 με.
tively 1.7, 2.8, and 3.2 times that of the reference paste. While this
This value was reduced to 340, 257, and 235 με when CF was
entrapped air could contribute to attenuating the sharp rise in
incorporated at dosages of 0.1, 0.15, and 0.2%, respectively. This
viscosity (Struble and Jiang 2004) caused by CF, it may lead to
corresponds to a reduction in autogenous shrinkage strains of 8, 31,
adverse effects on mechanical performance.
and 36% for the three respective CF addition rates.
The observed reduction in autogenous shrinkage deformations
Isothermal Calorimetry in pastes with CF may be associated with an internal curing effect
imparted by CF. The CF’s hydrophilic and hygroscopic features
Heat evolutions in the different paste mixtures are depicted in (discussed earlier) can provide a sort of internal water reservoir.
Fig. 10. The figure reveals two behaviors where the effect of The latter regulates the matrix’s internal moisture, which could
CF varies from insignificant during the first 7 h to a relatively slight have otherwise been destabilized by the water loss as cement hy-
increase in heat flow later. The figure also shows slightly higher and dration proceeds. On the other hand, the extremely small size of CF
broader silicate hydration peaks in the mixtures incorporating CF. coupled with the omnipresence of hydroxyl groups on its surface
This is further confirmed by the cumulative heat release whereby may promote CF interactions with the cementitious matrix such
the total released heat was slightly higher in all CF mixtures com- that CFs retain water and dispatch it to the matrix to partially re-
pared to that of the reference mixture. The mixture with 0.15% CF, plenish the emptying cement pores. This reduces self-desiccation
for instance, exhibited 7% higher cumulative heat release than that and attenuates early-age deformations, in consequence. This is
of the reference mixture. Such a trend is common in nanocellulose analogous to the well-reported effect of lightweight aggregates
(LWA) and superabsorbent polymers (SAP) on reducing shrinkage
deformations in cementitious systems. In this regard, conditional to
adequate CF dosage and dispersion, the effectiveness of CFs could
be even better. This can be justified by the fact that when CF is
used in this perspective, its advantage is twofold. This is because

Table 4. Some Fresh and Hardened Properties of Paste Mixtures Studied

for Autogenous Shrinkage
Splitting tensile strength
(MPa)
Slump Vicat final
Paste mixture (mm) setting time (min) 1 day 3 days 7 days
Ref. 265 418 1.52 2.35 3.18
0.1% CF 255 431 1.45 2.48 3.32
Fig. 10. Hydration heat flow and cumulative hydration heat release in 0.15% CF 245 439 1.50 2.54 3.71
paste mixtures 0.2% CF 240 442 1.39 2.42 3.68

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 Table 5. Fresh Properties of SCC Mixtures
Slump flow J-ring
V-funnel
Mix Air content (%) Density (kg=m3 ) Diameter (mm) T 500 (s) Diameter (mm) Blockage ratio T (s)
Ref. 1.0 2,315 785 1.83 770 0.86 2.13
0.10% CF 1.5 2,373 538 5.12 455 0.67 5.34
0.15% CF 3.0 2,316 320 — 310 0.60 14.75
0.20% CF 3.1 2,320 305 — 300 0.55 20.34

1990). Also, the drop in fc in paste mixtures can be attributed to the

increased likelihood of filament agglomeration (when CF content
increases) as supported by our microstructural analysis addressed in
the next section.
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In contrast to f c , the results of flexural strength (ffl ) of cement

pastes illustrated in Fig. 13 for both curing regimes reveal that the
addition of CF enhanced the flexural capacity—with higher im-
provements obtained under the sealed curing condition. The refer-
ence mixture, for instance, had comparable strengths under both
curing regimes. CF mixtures, however, showed higher ffl in sealed
curing than in moist curing. For the three CF dosages (0.1, 0.15,
and 0.2%), the improvements in f fl under the moist curing condi-
tion were 10, 25, and 28%, respectively, relative to reference.
Fig. 11. Early-age deformations in paste mixtures For the sealed curing, this corresponded to 19, 34, and 38%, respec-
tively, relative to the corresponding reference. These results suggest
that the improvement in ffl can possibly be linked to a combined
effect of (1) CF acting as nanoreinforcement owing to CF’s fibrillar
the filaments, additional to their effect on internal curing, may co- morphology and (2) CF serving as an internal curing agent for its
laterally increase the matrix tensile capacity through filament bridg- water affinity and retention/release capacity. This can curtail self-
ing, fracture, or pullout. Evidence for this interpretation was found desiccation, thereby leading to a volumetrically stable matrix as
in the splitting-tensile strength (fsp ) tests conducted (parallel to the supported by the autogenous shrinkage measurements.
autogenous shrinkage measurements) at 1, 3, and 7 days. Results However, while internal curing can contribute to explaining the
from those tests indicated that while no effect of CF was noticed on increased ffl of dry-sealed CF specimens relative to that of their
the 1-day strength, increases in f sp of 8 and 17% (relative to the reference, the reduced f fl measured in the moist condition for all
reference) were recorded at 3 and 7 days, respectively, in the specimens relative to their counterparts in the dry condition sug-
mixture with 0.15% CF, for instance (Table 4). gests that another phenomenon may prevail. This is because if
internal curing alone dominates the increase in f fl in the sealed
curing regime, it must do so or even better in the moist curing re-
Mechanical Properties
gime (when water is supplied internally and externally).
The compressive strength (f c ) results for all paste mixtures are de- In fact, the reduction of ffl in moist-cured specimens is attrib-
picted in Fig. 12. The figure indicates that in cement pastes, the utable to the excessive water saturation under this condition. Owing
addition of CF adversely affected fc under both curing regimes to the hygroscopic nature of CF, its moisture content can consid-
(moist and sealed). Furthermore, the reduction in f c was exacer- erably influence the mechanical properties of CF-cement compo-
bated as CF concentration increased. This can be traced to the sites. This is due to the well-reported effect of water saturation
air entrainment caused by the inclusion of CF as indicated earlier. on reducing the f fl of cementitious matrices incorporating natural
Such a reduction in f c was also reported for macrocellulose fibers fibers. Onuaguluchi and Banthia (2016), for instance, recorded an
owing to the amount of entrapped air (Soroushian and Marikunte 18–51% decrease in the ffl of natural fiber–cement systems

Fig. 12. Compressive strength (f c ) in pastes: (a) moist curing; (b) sealed curing

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 Fig. 13. Flexural strength (ffl ) of paste mixtures at 28 days
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Fig. 15. SEM image of a paste mixture with 0.15% CF

subjected to water saturation. This reduction is attributable to the

deterioration of the interfibrillar hydrogen bonds as well the fiber-
matrix interfacial bonds. This softens the fibers and weakens their
bonds with the matrix. As a result, the fibers mainly fail in pullout
(Coutts and Kightly 1984). The effect of moisture on the f fl of
cement systems with natural fibers has also been reported by
El-Ashkar et al. (2007) who found that natural fiber–cement mor-
tars dried in an oven exhibited higher f fl than those cured in air or
in water.

Microstructural Analysis
Microstructure investigations conducted using FEG-SEM on fresh
fractured paste samples revealed that CFs adhere well to the struc-
ture of the cementitious matrix. Fig. 14 shows several CFs ce-
mented into the CSH from one side and connected to parts of
the matrix from another side. The bottom of the figure also shows Fig. 16. SEM image of a paste mixture with 0.2% CF
several CFs well integrated in the matrix while bridging two parts
of the hydrated system and interfering with matrix pores. The ad-
herence of CF in the matrix is further supported by the SEM image The high surface area of CF and its extremely small size render
of Fig. 15. Moreover, Fig. 16 shows few CFs with protruding ends, the dispersion a difficult task, particularly as CF dosage increases.
which may have been cut during specimen fracture. The figure This consequently jeopardizes mechanical performance (particu-
shows a filament in the middle with an indented cross section, larly in compression) and may result in the reduction in f c observed
which seems to support the hygroscopic character of CF. The in- in paste mixtures. Under compression, CF entanglements such as
teraction of CFs with the hydrated system may contribute to ex- the ones depicted in Fig. 17(b) lead to increasing the porous net-
plaining the enhancement in mechanical properties, particularly work, thereby reducing f c . However, this adverse effect may not
f sp and ffl in CF-containing cement systems—elaborated in the be the same in flexural loading, where pulling out the entangled
previous section. On the other hand, Fig. 17(a) shows some spots filaments or fracturing them necessitates additional energy.
in the mixture with 0.2% CF, where CF clumps were observed. This builds up the matrix fracture resistance through the FRC
mechanism.

Results and Discussion for Concrete Mixtures

Flow Properties and Rheology

The results of fresh properties of the tested SCC mixtures are pre-
sented in Table 5. Data in the table indicate that the addition of CF
significantly altered mixture workability. A reduction in the flow
diameter (slump and J-ring) of more than 50% relative to the refer-
ence mixture and a significant increase in flow time (T 500 and
V-funnel times) were observed for CF additions of 0.15 and
0.2%. This reveals that CFs considerably altered mixture workabil-
ity and viscosity. This is also confirmed by rheological measure-
ments, which show that the addition of CF significantly increased
0
the evolution of the shear stress (τ ) versus shear rate (γ ) for all
Fig. 14. SEM image of a paste mixture with 0.1% CF
tested SCC mixtures (Fig. 18). This is accompanied by a significant

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Fig. 17. SEM image of a paste with 0.2% CF: (a) CF agglomeration spots; (b) CF entanglements

increase in the yield stress (τ 0 ) and plastic viscosity (μpl ). For CF pulverized or streamlined in the direction of flow, thereby leading
dosages of 0.1, 0.15, and 0.2%, the values of τ 0 were, respectively, to the attenuated rise in viscosity.
2, 5, and 8 times greater than that of the reference mixture. This
reflects the increased stability and the consequent high energy nec-
essary to start the flow when CFs are used. Nonetheless, once the Mechanical Properties
flow starts, the increments in μpl are relatively smaller, as Fig. 18 Fig. 19 presents the results of the compressive strength (fc ) of all
shows. The figure indicates increments in μpl of 1.5, 1.8, and 2.1 concrete mixtures where the influence of CF varies from no effect
times that of the reference mix for CF dosages of 0.1, 0.15, and at 1 day, to a marginal effect at 7 days, and to a moderate effect (up
0.2%, respectively. These are, in fact, lower than the corresponding to 16% increase) at 28 days. It is observable that the trend of fc in
aforementioned increments in τ 0 . This indicates the reduced mix- concrete mixtures is opposite to the decreasing trend noticed in
ture resistance to flow once the latter starts. cement pastes. This could be attributable to the fact that the fine
The observed trend of a sharp increase in τ 0 while μpl remained and coarse aggregates in concrete mixtures may have partially con-
relatively attenuated is often associated with high apparent viscos- tributed to increasing the shear mixing energy (imparted by only
0 0
ity (μapp ) at low values of γ , but low μapp as γ increases. Such a the mixer in the case of pastes). The effect of aggregates and the
behavior describes a high degree of pseudoplasticity (or shear thin- overall gradation of mixture constituents on increasing the shear
ning behavior), which is an interesting feature in flowable concrete. mixing energy can favor disintegrating CF clumps and/or aligning
0
This is because the increased μapp at low values of γ contributes to them in the flow direction. This promotes CF dispersion, which in
maintaining mixture constituents in suspension (hence more turn, contributes to the improvement in f c . This is consistent with
homogenous and stable mixtures). On the other hand, the attenu- the observations made in the previous section on CF-concrete mix-
0
ated μapp at high values of γ facilitates pumping and consolidation tures exhibiting a high degree of shear thinning behavior, where
0
(Ghio and Monteiro 1997). Such a rheological response in mixtures μapp was high at low values of γ (due to the propensity of CF
with CF suggests that the high τ 0 is attributed to the hydrophilic to water and to the formation of CF networks), but decreased with
0
nature of CF, leading to moisture absorption, and to the high aspect increasing γ (due to the breakage of filament networks and/or
ratio and flexibility of CFs, leading to the creation of filament net- alignment of individual fibrils in the direction of flow). The shear
0
works. This increases the viscosity buildup at low levels of γ . At thinning behavior imparted by CF increases the mixture’s ability to
0
high levels of γ , however, CF networks are more likely to be either

Fig. 18. Flow curves fitted to Bingham model for SCC mixtures Fig. 19. Compressive strength (f c ) of SCC mixtures

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 Fig. 20. Splitting-tensile strength (fsp ) of SCC mixtures
Fig. 22. Energy-absorption capacity of SCC mixtures
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maintain its variable-density constituents in suspension and re-

duces their inherent tendency to segregation. This fosters mixture plateauing of the corresponding load-deflection responses. Conse-
homogeneity and stability and enhances, in consequence, the prop- quently, the energy-absorption capacity depicted in Fig. 22 shows
erties of the hardened product, including f c . While the decrease in that the addition of CF at dosages of 0.1, 0.15, and 0.2% enhanced
the f c of pastes was attributed to the air entrainment and poor the energy-absorption capacity of the reference specimen by 33, 68,
dispersion of CF, the latter appears to be more influential because and 96%, respectively.
air entrainment by CF was observed in paste and concrete mixtures It is observable that whereas the ffl reached a peak value at the
alike. As such, the HRWRA (used in concrete mixtures but not in CF dosage of 0.15%, higher energy-absorption capacity was re-
pastes) may have positively affected the f c of concrete mixtures in corded at 0.2% CF. This suggests that, under flexural loading,
two ways: the first through dispersing CF, particularly when a sus- CFs can slightly influence the post-peak behavior by withstanding
pension of CF-water-HRWRA was prepared and homogenized for some tensile stresses little beyond the ultimate load so as to
that purpose prior to introduction to the mixer, and the second partially enhance sustaining the peak load for some extra micro-
through deflocculating cement flocks, thereby fostering cement deflections. Consequently, the enhanced energy-absorption capac-
dispersion and increasing the degree of cement hydration. ity imparted by CF was reflected by an increase in the peak
The effect of CFs on the mechanical properties of concrete is displacement by up to 43% above the plain SCC.
more pronounced in the splitting-tensile strength (fsp ) and flexural The increased energy-absorption capacity and the resulting in-
capacity (f fl ), in which the filaments are more likely to be solicited creased peak displacement with higher CF dosage while the f fl was
to serve as nanoreinforcements. Fig. 20 reveals increases in fsp of relatively low can be juxtaposed to what is often encountered in
11, 26, and 34% (above the reference SCC) for the three respective FRC with macrofibers. In FRC with macrofibers, the flexural
CF dosages (0.1, 0.15, and 0.2%). These observations are further capacity (peak load or rupture strength) is often sensitive to fc ,
supported by the results of ffl and the energy-absorption capacity whereas the postpeak behavior, however, is rather influenced by
(toughness) depicted in Figs. 21 and 22, respectively. Results the strengthening and toughening effects imparted by the FRC
from the four-point flexural tests (Fig. 21) indicate that the stiffness mechanism (Altoubat et al. 2016). The strengthening and toughen-
of all CF incorporating specimens was higher than that of the refer- ing effects in FRC are governed by fiber bridging, the fiber/matrix
ence and that the incorporation of CF at dosages of 0.1, 0.15, and interfacial bond, and fiber pullout (Lin et al. 2009). These are
0.2% increased the load-carrying capacity of the plain SCC by 9, known to consume increasing fracture energy depending on fiber
22, and 13%, respectively. characteristics, particularly, length, tensile capacity, bond with the
On the other hand, Figs. 21 and 22 indicate some toughening matrix, and fiber count.
effects imparted by CF. The reference specimen failed at a rela- In spite of the extended CF aspect ratio as compared to other
tively lower load than all specimens containing CF, and the drop nanocellulose particles, the filaments are extremely short when
in its load-carrying capacity was sharp, as expected. Specimens compared to the conventional fibers used in FRC. This alters
with CF, however, sustained the peak load for some additional the fracture behavior of CF-reinforced concrete in contrast to con-
range of microdeflections prior to failure as evidenced by the ventional FRC. As such, in light of the results of the f fl and tough-
ness presented in Figs. 21 and 22, respectively, it is possible that the
following scenarios prevail in the fracture behavior in the tested
SCC mixtures: Firstly, in the case of the SCC with 0.1% CF,
for instance, it can be perceived that once concrete is cracked,
the insufficient CF length and fiber count fail to transfer tensile
stresses across the matrix microcracks. Consequently, the concrete
composite fractures. Secondly, in the specimen with 0.15% CF, it is
possible that the slightly higher fiber count allows the transfer of
some tensile stresses across the microcracks before they become
macrocracks. This instantaneously delays the loss of the load-
carrying capacity but cannot alter its sharp drop once started.
Finally, in the specimen with 0.2% CF, it can be perceived that
the relatively higher fiber count may have allowed the transfer
of more tensile stresses across the microcracked section. This re-
Fig. 21. Load-deflection response for SCC mixtures at 28 days
sults in the observed delayed failure (as more energy is required to

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Fig. 25. SEM image illustrating the presence of CFs in the ITZ in the
Fig. 23. SEM image of a fractured SCC specimen 0.2% CF SCC with 0.15% CF

Fig. 24. SEM image illustrating the presence of CFs in the ITZ in the
SCC with 0.1% CF Fig. 26. SEM image illustrating the presence of CFs in the ITZ in the
SCC with 0.2% CF

pull the filaments out from the cracked surfaces) and reflects the
composite’s relatively increased fracture resistance. matrix (Ollivier et al. 1995; Wang et al. 2009; Erdem et al.
Nonetheless, the toughening effect imparted by CF remains re- 2012). This is generally associated to the wall effect, in which
strained by the CFs’ size. While the filaments’ micrometric size the aggregates appear locally flat relative to the cement grains,
may allow bridging nano/microcracks, the formation of macro- which disrupts cement packing (Scrivener et al. 2004), or to the
cracks causes an abrupt matrix rupture. As a result, the degradation microbleeding effect that leads to the accumulation of mixture
in the load-carrying capacity (once it starts) has never been gradual water beneath the aggregates during consolidation (Goldman
(in any CF-containing specimen) as the typical behavior encoun- and Bentur 1992). This makes the ITZ the weakest link of the mi-
tered in conventional FRC. Hence, a blend of CF and macrofibers crostructural system, where cracking initiates, and thus it has a phe-
is expected to possibly result in a synergetic effect, such that both nomenal effect on the mechanical and transport properties of
prepeak and postpeak behaviors are improved. concrete (Nemati et al. 1998; Wong et al. 2009). In this regards,
the addition of CFs appears to reinforce the ITZ, thereby contrib-
uting to the improved mechanical properties. This could substan-
Microstructural Analysis tiate the enhancement in f sp and ffl in CF mixtures elaborated
earlier.
The microstructure investigations of concrete mixtures are shown
in Figs. 23–26. Fig. 23 shows a mixture with 0.2% CF, exhibiting
several CFs with their fibrillar morphology quite evident, several Conclusions
protruding ends of CFs that may have been cut during sample frac-
turing, and a set of traces of filament pullout. This indicates a This study investigated the influence of a new type of nanocellulose
potential underlying filament bridging/fracturing mechanism con- materials, namely cellulose filaments, on the performance of ce-
tributing to enhancing the mechanical performance. On the other ment and concrete systems. The effects of CF addition at 0, 0.1,
hand, Figs. 24–26 show the presence of several CFs in the inter- 0.15, and 0.2% by weight on the properties of cement pastes
facial transition zone (ITZ) in the SCC mixtures with 0.1, 0.15, and and SCC mixtures were examined. In paste systems, the mechani-
0.2% CF, respectively. The ITZ is generally perceived to have lower cal properties were examined in a function of the curing regime
structural properties, much coarser pores, and easily cleavable (moist versus sealed). The results indicated that CFs altered mixture
highly soluble CH crystals compared to the bulk cementitious rheology and improved the stability of SCC mixtures owing to CF’s

© ASCE 04018109-12 J. Mater. Civ. Eng.

J. Mater. Civ. Eng., 2018, 30(6): 04018109

 hydrophilicity coupled with its high aspect ratio and flexibility. ASTM. (2013). “Standard test methods for time of setting of hydraulic
The improved mixture stability contributed to enhancement of cement by Vicat needle.” ASTM C191-13, West Conshohocken, PA.
the hardened product. ASTM. (2014a). “Standard practice for mechanical mixing of hydraulic
Results from the mechanical performance of cement pastes cement pastes and mortars of plastic consistency.” ASTM C305-14,
West Conshohocken, PA.
revealed that the compressive strength was negatively affected. This
ASTM. (2014b). “Standard specification for flow table for use in tests of
was traceable to the air entrainment and the formation of filament hydraulic cement.” ASTM C230/C230M-14, West Conshohocken, PA.
clumps as CF dosage increased. However, the flexural strength in ASTM. (2014c). “Standard test method for flexural strength of hydraulic
all CF paste mixtures was higher and improvement of up to 25% cement mortars.” ASTM C348-14, West Conshohocken, PA.
relative to the plain mixture was recorded. In SCC mixtures, ASTM. (2014d). “Standard test method for length change of hardened
all mechanical properties were improved. Relative to the plain hydraulic-cement mortar and concrete.” ASTM C157/C157M-08, West
SCC, strength improvement of up to 16% (in compression), Conshohocken, PA.
34% (in splitting tension), 22% (in flexure), and 96% (in energy ASTM. (2014e). “Standard test method for passing ability of self-
absorption) were recorded. The enhanced energy-absorption capac- consolidating concrete by J-ring.” ASTM C1621/C1621M-14, West
ity imparted by CF was reflected by an increase in the peak Conshohocken, PA.
ASTM. (2014f). “Standard test method for slump flow of self-consolidating
Downloaded from ascelibrary.org by NIEC Delhi Admin on 09/03/21. Copyright ASCE. For personal use only; all rights reserved.

displacement by up to 43% above the plain concrete mixture. This

implies a higher strain capacity, which is attractive for applications concrete.” ASTM C1611/C1611M-14, West Conshohocken, PA.
ASTM. (2015). “Standard test method for air content of hydraulic cement
where structures are required to exhibit such behavior prior to fail-
mortar.” ASTM C185-15, West Conshohocken, PA.
ure, such as in impact- and blast-resisting structures. The improved ASTM. (2016a). “Standard specification for chemical admixtures for
mechanical performance in paste and concrete mixtures incorporat- concrete.” ASTM C494/C494M-16, West Conshohocken, PA.
ing CF can be attributed to the following mechanisms: ASTM. (2016b). “Standard test method for compressive strength of cylin-
1. An internal curing effect, in which CFs act as internal water drical concrete specimens.” ASTM C39/C39M-16, West Conshohocken,
reservoirs to attenuate self-desiccation and reduce early-age de- PA.
formations, thereby leading to improved strength. This is sup- ASTM. (2016c). “Standard test method for compressive strength of hy-
ported by the results of the autogenous shrinkage assessment, in draulic cement mortars.” ASTM C109/C109M-16, West Conshohocken,
which the addition of CF at 0.1, 0.15, and 0.2% reduced the PA.
autogenous shrinkage strains of the plain system at 7 days ASTM. (2016d). “Standard test method for flexural strength of concrete
by 8, 31, and 36%. (using simple beam with third-point loading).” ASTM C78/C78M-16,
West Conshohocken, PA.
2. A nanoreinforcing effect, in which CFs were found to adhere to
ASTM. (2017). “Standard test method for measurement of heat of hydra-
the structure of the cementitious matrix and integrate with the
tion of hydraulic cementitious materials using isothermal conduction
hydrated system as supported by the microstructural investiga- calorimetry.” ASTM C1702-17, West Conshohocken, PA.
tions. For SCC mixtures, the results showed that the CFs’ na- Aziz, M. A., Paramasivam, P., and Lee, S. L. (1981). “Prospects for
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effect. In this case, the CFs’ hydrophilicity and fibrillar mor- Lightweight Concr., 3(2), 123–132.
phology contributed to improving the mechanical properties Banthia, N., Moncef, A., Chokri, K., and Sheng, J. (1994). “Micro-fiber
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Acknowledgments Boldizar, A., Klason, C., Kubat, J., Naslund, P., and Shah, P. (1987).
“Prehydrolyzed cellulose as reinforcing filler for thermoplastics.”
This project is jointly supported by a Cooperative Research and
Int. J. Polym. Mater., 11(4), 229–262.
Development (CRD) grant from the Natural Sciences and Brinchi, L., Cotana, F., Fortunati, E., and Kenny, J. M. (2013). “Production
Engineering Research Council of Canada (NSERC), Canada Vanier of nanocrystalline cellulose from lignocellulosic biomass: Technology
Graduate Scholarship (CGS) program award no: 360284, Kruger and applications.” Carbohyd. Polym., 94(1), 154–169.
Biomaterials, Inc. (QC, Canada), and Euclid Chemicals. The Cao, Y., Zavaterri, P., Youngblood, J., Moon, R., and Weiss, J. (2015). “The
authors are grateful for the financial support from all of these influence of cellulose nanocrystal additions on the performance of
partners. cement paste.” Cem. Concr. Compos., 56, 73–83.
Chung, D. D. L. (2000). “Cement reinforced with short carbon fibers—
A multifunctional material.” Composites, Part B, 31(6–7), 511–526.
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